Impact of Solution Chemistry and Particle Anisotropy on the Collective Dynamics of Oriented Aggregation
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Univ. of Washington, Seattle, WA (United States)
- Washington State Univ., Pullman, WA (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
While oriented aggregation (OA) of particles is a widely recognized mechanism of crystal growth, the impact of many fundamental parameters, such as crystallographically distinct interfacial structures, solution composition, and nanoparticle morphology on the governing mechanisms and assembly kinetics are largely unexplored. Thus, the collective dynamics of systems exhibiting OA has not been predicted. In this context, we investigated the structure and dynamics of boehmite aggregation as a function of solution pH and ionic strength. Cryogenic transmission electron microscopy reveals that boehmite nanoplatelets assemble by oriented attachment on (010) planes. The coagulation rate constants obtained from dynamic light scattering during the early stages of aggregation span seven orders of magnitude and cross both the reaction-limited and diffusion-limited regimes. Combining a simple scaling analysis with calculations for stability ratios and rotational/translational diffusivities of irregular particle shapes, the effects of orientation for irregular-shaped particles on the early stages of aggregation is understood via angular dependence of van der Waals, electrostatic, and hydrodynamic interactions. Using Monte Carlo simulations, we discovered that a simple geometric parameter, namely the contact area between two attaching nanoplatelets, presents a useful tool for correlating nanoparticle morphologies to the emerging larger-scale aggregates, hence explaining the unusually high fractal dimensions measured for boehmite aggregates. Our results on nanocrystal transport and interactions provide insights towards the predictive understanding of nanoparticle growth, assembly, and aggregation, which will important critical challenges in the developing synthesis strategies for nanostructured materials, understanding the evolution of geochemical reservoirs, and addressing many environmental problems.
- Research Organization:
- Energy Frontier Research Centers (EFRC) (United States). Interfacial Dynamics in Radioactive Environments and Materials (IDREAM); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Biological and Environmental Research (BER)
- Grant/Contract Number:
- AC05-76RL01830; AC05-00OR22725
- OSTI ID:
- 1558377
- Alternate ID(s):
- OSTI ID: 1775252
- Report Number(s):
- PNNL-SA-138292
- Journal Information:
- ACS Nano, Vol. 12, Issue 10; ISSN 1936-0851
- Publisher:
- American Chemical Society (ACS)Copyright Statement
- Country of Publication:
- United States
- Language:
- English
Web of Science
Interplay between Short- and Long-Ranged Forces Leading to the Formation of Ag Nanoparticle Superlattice
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journal | June 2019 |
Quantized grain boundary states promote nanoparticle alignment during imperfect oriented attachment | preprint | January 2020 |
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